Abstract
The aN and aIINH hyperfine splitting constants of pyridinyl are poorly reproduced by INDO molecular orbital calculations if assuming a planar geometry for the radical. A much better agreement with experiment has been found by evaluating these constants from vibronic wavefunctions even though at a semiquantitative level. The effects of substituents and of solvent polarity on the hyperfine splittings of pyridinyls are also discussed.
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